[Objectives] To establish the process flow of preparation of Wufang Babu Poultice and the identification method of thin layer chromatography (TLC). [Methods] For the forming process of Wufang Babu Poultice, the prepar...[Objectives] To establish the process flow of preparation of Wufang Babu Poultice and the identification method of thin layer chromatography (TLC). [Methods] For the forming process of Wufang Babu Poultice, the preparation method of mixed pharmaceutical powder with suitable pharmaceutical excipients was adopted. Qualitative identification of medicinal materials in Wufang Babu Poultice (Strychni Semen, Rhei Radix Et Rhizoma, Dipsaci Radix, and Angelicae Sinensis Radix) was carried out by TLC. [Results] Mixed pharmaceutical powder mixed with glycerol, gelatin and other pharmaceutical excipients can be prepared for forming. The test solution chromatography of each medicinal material (Strychni Semen, Rhei Radix et Rhizoma, Dipsaci Radix, Angelicae Sinensis Radix) showed pigment spots of the same color at the same position as its corresponding control medicinal materials and reference chromatography, and the display was clear. [Conclusions] The preparation process is simple and feasible, and can be used as the forming process of Wufang Babu Poultice. The TLC determination method is simple to operate, has good specificity, and has no effect on negative results, and can be used for identification of Wufang Babu Poultice.展开更多
During the development of hot dry rock,the research on thermal fatigue damage caused by thermal shock of cold and heat cycles is the basis that ensures the long-term utilization of geothermal resources,but there are n...During the development of hot dry rock,the research on thermal fatigue damage caused by thermal shock of cold and heat cycles is the basis that ensures the long-term utilization of geothermal resources,but there are not enough relevant studies at present.Based on this,the thermal damage tests of granite at different temperatures(250,350,450°C)and quenching cycles(1,5,10,15 cycles)were carried out.Preliminary reveals the damage mechanism and heat transfer law of the quenching cycle effect on hot dry rock.The results show that with the increase of temperature and cycles,the uneven thermal expansion of minerals and the thermal shock caused by quenching promote the crack development of granite,resulting in the decrease of P-wave velocity,thermal conductivity and uniaxial compressive strength of granite.Meanwhile,the COMSOL was used to simulate the heat transfer of hot dry rock under different heat treatment conditions.It concluded that the increase in the number of quenching cycles reduced the heat transfer capacity of the granite,especially more than 10 quenching cycles,which also reflects that the thermal fatigue damage leads to a longer time for the temperature recovery of the hot dry rock mass.In addition,the three-dimensional nonlinear fitting relationship among thermal conductivity,temperature and cycle number was established for the first time,which can better reveal the change rule of thermal conductivity after quenching thermal fatigue effect of hot dry rock.The research results provide theoretical support for hot dry rock reservoir reconstruction and production efficiency evaluation.展开更多
Background Burn-out among doctors threatens their own health, and that of their patients. To identify risk factors of the doctor burn-out is vital to improving their health and increasing the quality of healthcare s...Background Burn-out among doctors threatens their own health, and that of their patients. To identify risk factors of the doctor burn-out is vital to improving their health and increasing the quality of healthcare services. This study aims to explore the relationship between work-family confict (WFC) and burn-out among Chinese doctors and the mediating role of coping styles in this relationship.Methods A cross-sectional survey was conducted in China, with a questionnaire packet which consisted of the Chinese Maslach Burnout Inventory (CMBI), WFC Scale and the Simplifed Coping Style Questionnaire (SCSQ). A total of 2530 doctors participated in the survey. Correlation analysis was performed to explore the relationship between CMBI, WFC and SCSQ scores. A linear regression model was set to determine the mediating role of coping styles on the relationship between WFC and burn-out.Results Doctors who had higher scores on work interfering with family confict, reported more emotional exhaustion (r=0.514, P〈0.001) and had a sense of accomplishment (r= 0.149, P〈0.001). Simultaneously, family interfering with work (FIW) was positively associated with all dimensions of burn-out (r=0.213, 0.504, 0.088, respectively, P〈0.001). Coping styles had partial, complete and even mediating effects on the relationship between WFC and burn-out among Chinese doctors.Conclusions WFC was correlated with burn-out, and coping style was a mediator in this relationship among Chinese doctors. Coping style was a positive resource against burn-out.展开更多
With the explosive growth of Internet information, it is more and more important to fetch real-time and related information. And it puts forward higher requirement on the speed of webpage classification which is one o...With the explosive growth of Internet information, it is more and more important to fetch real-time and related information. And it puts forward higher requirement on the speed of webpage classification which is one of common methods to retrieve and manage information. To get a more efficient classifier, this paper proposes a webpage classification method based on locality sensitive hash function. In which, three innovative modules including building feature dictionary, mapping feature vectors to fingerprints using Localitysensitive hashing, and extending webpage features are contained. The compare results show that the proposed algorithm has better performance in lower time than the naive bayes one.展开更多
Talaroclauxins A and B(1 and 2),two novel duclauxin hybrids,were obtained from Talaromyces stipitatus,along with three new(3-5)and one known analogue(6).Their structures were determined by NMR spectroscopy,HRESIMS,sin...Talaroclauxins A and B(1 and 2),two novel duclauxin hybrids,were obtained from Talaromyces stipitatus,along with three new(3-5)and one known analogue(6).Their structures were determined by NMR spectroscopy,HRESIMS,single-crystal X-ray diffraction,and quantum chemical calculations.Compound 1 is the first example of duclauxin-ergosterol hybrid featuring an unprecedented dodecacyclic ring system formed via a[4+2]cycloaddition,while compound 2,bearing an unusual 6/6/6/5/6/6/6/6 ring system,is a new member of the rare duclauxin-polyketide hybrid class of natural products.Plausible biosynthetic pathways for 1-6 are proposed.Compound 5 displayed moderate neuroprotective effects in glutamate sodium-induced SH-SY5Y cells.展开更多
We reported the characterization of a novel brassicicene diterpene biosynthetic gene cluster,which contains a uniqueα-ketoglutarate-dependent dioxygenase(αKGD)enzyme,AbnI.Our findings revealed that AbnI demonstrates...We reported the characterization of a novel brassicicene diterpene biosynthetic gene cluster,which contains a uniqueα-ketoglutarate-dependent dioxygenase(αKGD)enzyme,AbnI.Our findings revealed that AbnI demonstrates remarkable substrate promiscuity and is capable of activating multiple sites on both 5-8-5 and 5-9-5 brassicicene skeletons,resulting in skeleton modifications and an unexpected ring system rearrangement.These results suggested the potential utility of AbnI as an enzymatic tool for terpene C-H functionalization.In addition,the catalytic mechanism of AbnI and its potential ecological implications were discussed.展开更多
Respiratory syncytial virus(RSV)is the major cause of bronchiolitis and pneumonia in young children and the elderly.There are currently no approved RSV-specific therapeutic small molecules available.Using high-through...Respiratory syncytial virus(RSV)is the major cause of bronchiolitis and pneumonia in young children and the elderly.There are currently no approved RSV-specific therapeutic small molecules available.Using high-throughput antiviral screening,we identified an oral drug,the prenylation inhibitor lonafarnib,which showed potent inhibition of the RSV fusion process.Lonafarnib exhibited antiviral activity against both the RSV A and B genotypes and showed low cytotoxicity in HEp-2 and human primary bronchial epithelial cells(HBEC).Time-of-addition and pseudovirus assays demonstrated that lonafarnib inhibits RSV entry,but has farnesyltransferase-independent antiviral efficacy.Cryo-electron microscopy revealed that lonafarnib binds to a triple-symmetric pocket within the central cavity of the RSV F metastable pre-fusion conformation.Mutants at the RSV F sites interacting with lonafarnib showed resistance to lonafarnib but remained fully sensitive to the neutralizing monoclonal antibody palivizumab.Furthermore,lonafarnib dose-dependently reduced the replication of RSV in BALB/c mice.Collectively,lonafarnib could be a potential fusion inhibitor for RSV infection.展开更多
Development of high-performance solid state luminescent carbon-based nanomaterials remains challenging.Here,strong blue-green fluorescent carbonized polymer dots(CPDs)from o-aminobenzenethiol and thiosalicylic acid(o ...Development of high-performance solid state luminescent carbon-based nanomaterials remains challenging.Here,strong blue-green fluorescent carbonized polymer dots(CPDs)from o-aminobenzenethiol and thiosalicylic acid(o ABT-TSA-CPDs)with an absolute photoluminescence quantum yield(PLQY)of 76%in solid state without matrix were synthesized.Through adjusting the reaction temperature and time,the PL centers were proved to be carbon core state and surface state associated to carbonyl group which was the source of strong fluorescence emission in solid state.The mechanism of the unique phenomenon of enhanced emission from ethanol solution(PLQY=7%)to powder(PLQY=76%)was investigated by analyzing the chemical properties and structures of o ABT-TSA-CPDs at different temperatures and o ABT-TSACPDs/PVC composites,and was confirmed as fixation of PL centers.展开更多
The dioxygen activation catalyzed by 4-hydorxylphenyl pyruvate dioxygenase(HPPD)were reinvestigated by using hybrid quantum mechanics/molecular mechanics(QM/MM)approaches at the B3LYP/6-311++G(d,p):AMBER level.These s...The dioxygen activation catalyzed by 4-hydorxylphenyl pyruvate dioxygenase(HPPD)were reinvestigated by using hybrid quantum mechanics/molecular mechanics(QM/MM)approaches at the B3LYP/6-311++G(d,p):AMBER level.These studies showed that this reaction consisted of two steps including the dioxygen addition/decarboxylation and hetero O-O bond cleavage,where the first step was found to be rate-determining.The former step initially runs on a septet potential energy surface(PES),then switches to a quintet PES after crossing a septet/quintet minimum energy crossing point(MECP)5-7M2,whereas the rest step runs on the quintet PES.The reliability of our theoretical predictions is supported by the excellent agreement of the calculated free-energy barrier value of 16.9 kcal/mol with available experimental value of 16-17 kcal/mol.The present study challenges the widely accepted view which holds that the O2activation catalyzed byα-keto glutamate(α-KG)dioxygenase mainly runs on the quintet PES and provides new insight into the catalytic mechanism ofα-KG dioxygenase and/or other related Fe(Ⅱ)-dependent oxygenase.展开更多
Noncovalentlycross-linkedpolymermaterials through healing,recycling,and reprocessing can reduce materials consumption and alleviate environmental pollution.However,it remains a huge challenge to fabricate super-strong...Noncovalentlycross-linkedpolymermaterials through healing,recycling,and reprocessing can reduce materials consumption and alleviate environmental pollution.However,it remains a huge challenge to fabricate super-strong noncovalently cross-linked polymer materials with mechanical strength comparable to high-performance engineering polymers.Herein,healable and reprocessable noncovalently cross-linked polymer compositeswith an unprecedented mechanical strength are fabricated by complexation of polyacrylic acid(PAA),polyvinylpyrrolidone(PVPON),and carbonized polymer dots(CPDs)(denoted as PAA-PVPON-CPDs).The incorporation of 15 wt%CPDs generates PAA-PVPON-CPDs compositeswith a tensile strength of∼158 MPa and Young’s modulus of∼8.2GPa.Servingas nanofillers,theCPDs can establish strong interactions with polymers in PAA-PVPON composites.The CPDs and the in situ-formed PAAPVPON nanoparticles work in concert to significantly strengthen the PAA-PVPON-CPDs composites to an unprecedented strength.The PAA-PVPON-CPDs composites exhibit excellent impact resistance and damage tolerance because of the high mechanical strength of the composites and the energy dissipation mechanism of the CPDs and PAA-PVPON nanoparticles.Moreover,the fractured PAA-PVPON-CPDs composites can be healed to restore their original mechanical strength.展开更多
Dendrobium plants are used commonly as tonic herbs and health food in many Asian countries, especially in China. Here we report the genetic map construction of two Dendrobium species with a double pseudo-testcross str...Dendrobium plants are used commonly as tonic herbs and health food in many Asian countries, especially in China. Here we report the genetic map construction of two Dendrobium species with a double pseudo-testcross strategy using random amplified polymorphic DNA (RAPD) and sequence-related amplified polymorphism (SRAP) markers. A F1 mapping population of 90 individuals was developed from a cross between D. officinale and D. hercoglossum. A total of 307 markers, including 209 RAPD and 98 SRAP, were identified and used for genetic linkage group (LG) analysis. The D. officinale linkage map consisted of 11 major linkage groups and 3 doublets, which covered 629.4 cM by a total of 62 markers with an average locus distance of 11.2 cM between two adjacent markers. The D. hercoglos- sum linkage map contained 112 markers mapped on 15 major and 4 minor linkage groups, spanning a total length of 1,304.6 cM with an average distance of I 1.6 cM between two adjacent markers. The maps constructed in this study covered 92.7% and 82.7% of the D. hercoglossum and D. officinale genomes respectively, providing an important basis for the mapping of horticultural and medicinal traits and for the application of marker-assisted selection in Dendrobium breeding program.展开更多
Five novel heterodimers of cytochalasan and ergosterol,ergochaeglobosins A—E,were isolated from an endophytic fungus Chaetomium globosum P2-2-2.Ergochaeglobosin A(1) possesses an unprecedented 5/6/13/6/5/6/6/6 fused ...Five novel heterodimers of cytochalasan and ergosterol,ergochaeglobosins A—E,were isolated from an endophytic fungus Chaetomium globosum P2-2-2.Ergochaeglobosin A(1) possesses an unprecedented 5/6/13/6/5/6/6/6 fused octacyclic ring system,and ergochaeglobosins B(2) and C(3) form a unique 5/6/13/6/6/6/6/5 fused octacyclic ring system,whereas ergochaeglobosins D(4) and F(5) are the first cytochalasan heterodimers formed via a N-1′/C-3′′single bond.Their structures with absolute configurations were established by extensive spectroscopic analyses,single-crystal X-ray diffraction,and ECD calculations.The plausible biogenetic pathway of 1—5 was postulated.Compound 1 exhibited inhibitory effects against ConA-induced T cells and LPS-induced B cells proliferation with IC50 values of 19.2 and 14.1μmol/L,respectively.Co-treatment of 3(20μmol/L)with TRAIL(150 ng/mL)could significantly decrease the cell viability of A549 by 24.9%comparing with monotherapy of 3(20μmol/L).展开更多
Quasi-2D perovskites have been demonstrated to be competitive materials in the photodetection fields due to the enhanced moisture stability by large organic cations.However,as the increasing demands of modern technolo...Quasi-2D perovskites have been demonstrated to be competitive materials in the photodetection fields due to the enhanced moisture stability by large organic cations.However,as the increasing demands of modern technology,it is still challenging to combine the flexibility with the capability of weak light detection in a low-cost way.Here,amides,carboxylic acids,and anhydrides groups-rich carbonized polymer dots(CPDs)were employed to fll in the perovskite grain boundaries,which can passivate the point defects of perovskite by coordinating with the unbonded Pb atoms,and reduce the leakage current.Weak light detection capability was demonstrated by directly resolving light with an intensity of 10.1 pW cm^(-2).More importantly,the stretchable polymer chains on CPDs strongly interact with perovskite ions through multiple supramolecular interactions,and extend the stretchable properties to the perovskite/CPDs composites,which can maintain the integral structure stability during the deformation of perovskite crystals and restricted any crack by releasing the flm strain.Our fabricated devices show extraordinary flexible stability in the bending-dependent response tests.The viscoelasticity of CPDs improves the bending stability of the flexible quasi-2D perovskite photodetectors,and device performance shows no degradation after bending 10000 times,comparable or even outperforming the dominating flexible photodetectors.展开更多
Sensitive differentiation of an enantiomer from its mirror image(ie,enantiodifferentiation),a perennial challenge for pharmaceutical production and disease diagnosis,is technically limited by the weak optical activity...Sensitive differentiation of an enantiomer from its mirror image(ie,enantiodifferentiation),a perennial challenge for pharmaceutical production and disease diagnosis,is technically limited by the weak optical activity(OA)of enantiomers,mainly due to their dimensional mismatch with light wavelengths in the ultraviolet(UV)-visible region.Here we use silver chiral nanoparticles(Ag CNPs)with nominally sub-5 nm helical pitch(P)to amplify the OA of(20R,30R,40S)-riboflavin-50-phosphate sodium salts(RP),which have been found to indirectly affect metabolic processes,through the formation of an RP thin film(TF)covering a close-packed array of Ag CNPs.The OA of the RP in the deep-UV region can be amplified up to 80-fold,ascribed to the aggregation of RP in the TFs and the interactions between RP and the atomically chiral lattices at the CNPs'surfaces.The former contribution,not associated with the chiral Ag topographies,plays a dominant role by thickening the RP TFs,so that the observed amplification has no enantioselective dependence on the chirality of the Ag CNPs.This study extends progress in the sensitive detection of bio-enantiomers,which is highly desired for advanced bio-detection in disease diagnosis and production of single-enantiomer pharmaceuticals.展开更多
4-Hydroxyphenylpyruvate dioxygenase(HPPD)is an important target for both drug and pesticide discovery.As a typical Fe(II)-dependent dioxygenase,HPPD catalyzes the complicated transformation of 4-hydroxyphenylpyruvic a...4-Hydroxyphenylpyruvate dioxygenase(HPPD)is an important target for both drug and pesticide discovery.As a typical Fe(II)-dependent dioxygenase,HPPD catalyzes the complicated transformation of 4-hydroxyphenylpyruvic acid(HPPA)to homogentisic acid(HGA).The binding mode of HPPA in the catalytic pocket of HPPD is a focus of research interests.Recently,we reported the crystal structure of Arabidopsis thaliana HPPD(At HPPD)complexed with HPPA and a cobalt ion,which was supposed to mimic the pre-reactive structure of At HPPD-HPPA-Fe(II).Unexpectedly,the present study shows that the restored At HPPD-HPPA-Fe(II)complex is still nonreactive toward the bound dioxygen.QM/MM and QM calculations reveal that the HPPA resists the electrophilic attacking of the bound dioxygen by the trim of its phenyl ring,and the residue Phe381 plays a key role in orienting the phenyl ring.Kinetic study on the F381 A mutant reveals that the HPPD-HPPA complex observed in the crystal structure should be an intermediate of the substrate transportation instead of the pre-reactive complex.More importantly,the binding mode of the HPPA in this complex is shared with several well-known HPPD inhibitors,suggesting that these inhibitors resist the association of dioxygen(and exert their inhibitory roles)in the same way as the HPPA.The present study provides insights into the inhibition mechanism of HPPD inhibitors.展开更多
In this paper, we study stabilization for a Schoedinger equation, which is interconnected with a heat equation via boundary coupling. A direct boundary feedback control is adopted. By a detailed spectral analysis, it ...In this paper, we study stabilization for a Schoedinger equation, which is interconnected with a heat equation via boundary coupling. A direct boundary feedback control is adopted. By a detailed spectral analysis, it is found that there are two branches of eigenvalues: one is along the negative real axis, and the other is approaching to a vertical line, which is parallel to the imagine axis. Moreover, it is shown that there is a set of generalized eigenfunctions, which forms a Riesz basis for the energy state space. Finally, the spectrum-determined growth condition is held and the exponential stability of the system is then concluded.展开更多
基金Supported by Key R&D Plan of Guangxi Zhuang Autonomous Region(Guike AB20297010).
文摘[Objectives] To establish the process flow of preparation of Wufang Babu Poultice and the identification method of thin layer chromatography (TLC). [Methods] For the forming process of Wufang Babu Poultice, the preparation method of mixed pharmaceutical powder with suitable pharmaceutical excipients was adopted. Qualitative identification of medicinal materials in Wufang Babu Poultice (Strychni Semen, Rhei Radix Et Rhizoma, Dipsaci Radix, and Angelicae Sinensis Radix) was carried out by TLC. [Results] Mixed pharmaceutical powder mixed with glycerol, gelatin and other pharmaceutical excipients can be prepared for forming. The test solution chromatography of each medicinal material (Strychni Semen, Rhei Radix et Rhizoma, Dipsaci Radix, Angelicae Sinensis Radix) showed pigment spots of the same color at the same position as its corresponding control medicinal materials and reference chromatography, and the display was clear. [Conclusions] The preparation process is simple and feasible, and can be used as the forming process of Wufang Babu Poultice. The TLC determination method is simple to operate, has good specificity, and has no effect on negative results, and can be used for identification of Wufang Babu Poultice.
基金financially supported by National Natural Science Foundation of China(Nos.U2013603,52004167,52078477,51827901,and U1965203)Sichuan International Technological innovation Cooperation Project(No.2018HH0159)。
文摘During the development of hot dry rock,the research on thermal fatigue damage caused by thermal shock of cold and heat cycles is the basis that ensures the long-term utilization of geothermal resources,but there are not enough relevant studies at present.Based on this,the thermal damage tests of granite at different temperatures(250,350,450°C)and quenching cycles(1,5,10,15 cycles)were carried out.Preliminary reveals the damage mechanism and heat transfer law of the quenching cycle effect on hot dry rock.The results show that with the increase of temperature and cycles,the uneven thermal expansion of minerals and the thermal shock caused by quenching promote the crack development of granite,resulting in the decrease of P-wave velocity,thermal conductivity and uniaxial compressive strength of granite.Meanwhile,the COMSOL was used to simulate the heat transfer of hot dry rock under different heat treatment conditions.It concluded that the increase in the number of quenching cycles reduced the heat transfer capacity of the granite,especially more than 10 quenching cycles,which also reflects that the thermal fatigue damage leads to a longer time for the temperature recovery of the hot dry rock mass.In addition,the three-dimensional nonlinear fitting relationship among thermal conductivity,temperature and cycle number was established for the first time,which can better reveal the change rule of thermal conductivity after quenching thermal fatigue effect of hot dry rock.The research results provide theoretical support for hot dry rock reservoir reconstruction and production efficiency evaluation.
基金special fund for public welfare industry of health grant(200802150)(JSYRKJ2010-C1-001Jiangsu Provincial Medical Humanities and Social Science committee(No:JSYRKJ2010-C1-001)+1 种基金Philosophy and Social Science Special Project in Nanjing Medical University(No:2013NJZS40)Key Project supported by Medical Science and Technology Development Foundation Nanjing Department of Healt(No.YKK17246,YKK16241)
文摘Background Burn-out among doctors threatens their own health, and that of their patients. To identify risk factors of the doctor burn-out is vital to improving their health and increasing the quality of healthcare services. This study aims to explore the relationship between work-family confict (WFC) and burn-out among Chinese doctors and the mediating role of coping styles in this relationship.Methods A cross-sectional survey was conducted in China, with a questionnaire packet which consisted of the Chinese Maslach Burnout Inventory (CMBI), WFC Scale and the Simplifed Coping Style Questionnaire (SCSQ). A total of 2530 doctors participated in the survey. Correlation analysis was performed to explore the relationship between CMBI, WFC and SCSQ scores. A linear regression model was set to determine the mediating role of coping styles on the relationship between WFC and burn-out.Results Doctors who had higher scores on work interfering with family confict, reported more emotional exhaustion (r=0.514, P〈0.001) and had a sense of accomplishment (r= 0.149, P〈0.001). Simultaneously, family interfering with work (FIW) was positively associated with all dimensions of burn-out (r=0.213, 0.504, 0.088, respectively, P〈0.001). Coping styles had partial, complete and even mediating effects on the relationship between WFC and burn-out among Chinese doctors.Conclusions WFC was correlated with burn-out, and coping style was a mediator in this relationship among Chinese doctors. Coping style was a positive resource against burn-out.
文摘With the explosive growth of Internet information, it is more and more important to fetch real-time and related information. And it puts forward higher requirement on the speed of webpage classification which is one of common methods to retrieve and manage information. To get a more efficient classifier, this paper proposes a webpage classification method based on locality sensitive hash function. In which, three innovative modules including building feature dictionary, mapping feature vectors to fingerprints using Localitysensitive hashing, and extending webpage features are contained. The compare results show that the proposed algorithm has better performance in lower time than the naive bayes one.
基金the Program for Changjiang Scholars of Ministry of Education of the People's Republic of China(No.T2016088)the National Natural Science Foundation for Distinguished Young Scholars(No.81725021)+6 种基金the National Natural Science Foundation for Excellent Young Scholars(No.81922065)Innovative Research Groups of the National Natural Science Foundation of China(No.81721005)the National Natural Science Foundation of China(No.82173706)the Science and Technology Major Project of Hubei Province(No.2021ACA012)the Research and Development Program of Hubei Province(No.2020BCA058)the Academic Frontier Youth Team of HUST(No.2017QYTD19)the Integrated Innovative Team for Major Human Diseases Program of Tongji Medical College(HUST).
文摘Talaroclauxins A and B(1 and 2),two novel duclauxin hybrids,were obtained from Talaromyces stipitatus,along with three new(3-5)and one known analogue(6).Their structures were determined by NMR spectroscopy,HRESIMS,single-crystal X-ray diffraction,and quantum chemical calculations.Compound 1 is the first example of duclauxin-ergosterol hybrid featuring an unprecedented dodecacyclic ring system formed via a[4+2]cycloaddition,while compound 2,bearing an unusual 6/6/6/5/6/6/6/6 ring system,is a new member of the rare duclauxin-polyketide hybrid class of natural products.Plausible biosynthetic pathways for 1-6 are proposed.Compound 5 displayed moderate neuroprotective effects in glutamate sodium-induced SH-SY5Y cells.
基金financially supported by the National Key R&D Program of China(Nos.2021YFA0910500,2021YFA0910503)the National Natural Science Foundation of China(Nos.22277035,32000045 and 81973205)+4 种基金the Program for Changjiang Scholars of Ministry of Education of the People’s Republic of China(No.T2016088)the National Natural Science Foundation for Distinguished Young Scholars(No.81725021)the National Science and Technology Project of China(No.2018ZX09201001-001-003)Innovative Research Groups of the National Natural Science Foundation of China(No.81721005)the Fundamental Research Funds for the Central Universities(No.2020kfyXJJS043).
文摘We reported the characterization of a novel brassicicene diterpene biosynthetic gene cluster,which contains a uniqueα-ketoglutarate-dependent dioxygenase(αKGD)enzyme,AbnI.Our findings revealed that AbnI demonstrates remarkable substrate promiscuity and is capable of activating multiple sites on both 5-8-5 and 5-9-5 brassicicene skeletons,resulting in skeleton modifications and an unexpected ring system rearrangement.These results suggested the potential utility of AbnI as an enzymatic tool for terpene C-H functionalization.In addition,the catalytic mechanism of AbnI and its potential ecological implications were discussed.
基金supported by the Natural Science Foundation of Guangdong province(Grant no.2024A1515011589 to Q.Y.)the National Natural Science Foundation of China(Grant no.32000111 to Q.Y.,82170473 to J.S.)+3 种基金the Pearl River Talent Recruitment Program(Grant no.2019CX01Y422 to X.C.)the Guangzhou Laboratory(Grant no.SRPG22-002 to J.S.and X.C.,No.SRPG22-011 to W.P.and Q.Y.)the Basic and Applied Basic Research Projects of Guangzhou Basic Research Program(2023A04J0161 to Q.Y.,2021QN020451 to J.S.)the Young Elite Scientists Sponsorship Program by CAST(Grant no.2023QNRC001 to F.L.).
文摘Respiratory syncytial virus(RSV)is the major cause of bronchiolitis and pneumonia in young children and the elderly.There are currently no approved RSV-specific therapeutic small molecules available.Using high-throughput antiviral screening,we identified an oral drug,the prenylation inhibitor lonafarnib,which showed potent inhibition of the RSV fusion process.Lonafarnib exhibited antiviral activity against both the RSV A and B genotypes and showed low cytotoxicity in HEp-2 and human primary bronchial epithelial cells(HBEC).Time-of-addition and pseudovirus assays demonstrated that lonafarnib inhibits RSV entry,but has farnesyltransferase-independent antiviral efficacy.Cryo-electron microscopy revealed that lonafarnib binds to a triple-symmetric pocket within the central cavity of the RSV F metastable pre-fusion conformation.Mutants at the RSV F sites interacting with lonafarnib showed resistance to lonafarnib but remained fully sensitive to the neutralizing monoclonal antibody palivizumab.Furthermore,lonafarnib dose-dependently reduced the replication of RSV in BALB/c mice.Collectively,lonafarnib could be a potential fusion inhibitor for RSV infection.
基金supported financially by the National Science Foundation of China(Nos.22035001,21774041)Jilin University Science and Technology Innovative Research Team(No.2017TD-06)。
文摘Development of high-performance solid state luminescent carbon-based nanomaterials remains challenging.Here,strong blue-green fluorescent carbonized polymer dots(CPDs)from o-aminobenzenethiol and thiosalicylic acid(o ABT-TSA-CPDs)with an absolute photoluminescence quantum yield(PLQY)of 76%in solid state without matrix were synthesized.Through adjusting the reaction temperature and time,the PL centers were proved to be carbon core state and surface state associated to carbonyl group which was the source of strong fluorescence emission in solid state.The mechanism of the unique phenomenon of enhanced emission from ethanol solution(PLQY=7%)to powder(PLQY=76%)was investigated by analyzing the chemical properties and structures of o ABT-TSA-CPDs at different temperatures and o ABT-TSACPDs/PVC composites,and was confirmed as fixation of PL centers.
基金supported by the National Key R&D Program(No.2021YFD1700100)National Natural Science Foundation of China(Nos.21837001,21273089)+2 种基金the Open Project Fund of the Key Laboratory of the Pesticides and Chemical Biology of Central China Normal University(No.2018-A01)the Fundamental Research Funds for the Central Universitiesthe Fundamental Research Funds for the South-Central University for Nationalities(No.CZW20020)。
文摘The dioxygen activation catalyzed by 4-hydorxylphenyl pyruvate dioxygenase(HPPD)were reinvestigated by using hybrid quantum mechanics/molecular mechanics(QM/MM)approaches at the B3LYP/6-311++G(d,p):AMBER level.These studies showed that this reaction consisted of two steps including the dioxygen addition/decarboxylation and hetero O-O bond cleavage,where the first step was found to be rate-determining.The former step initially runs on a septet potential energy surface(PES),then switches to a quintet PES after crossing a septet/quintet minimum energy crossing point(MECP)5-7M2,whereas the rest step runs on the quintet PES.The reliability of our theoretical predictions is supported by the excellent agreement of the calculated free-energy barrier value of 16.9 kcal/mol with available experimental value of 16-17 kcal/mol.The present study challenges the widely accepted view which holds that the O2activation catalyzed byα-keto glutamate(α-KG)dioxygenase mainly runs on the quintet PES and provides new insight into the catalytic mechanism ofα-KG dioxygenase and/or other related Fe(Ⅱ)-dependent oxygenase.
基金supported by the National Natural Science Foundation of China(NSFC grant no.21935004).
文摘Noncovalentlycross-linkedpolymermaterials through healing,recycling,and reprocessing can reduce materials consumption and alleviate environmental pollution.However,it remains a huge challenge to fabricate super-strong noncovalently cross-linked polymer materials with mechanical strength comparable to high-performance engineering polymers.Herein,healable and reprocessable noncovalently cross-linked polymer compositeswith an unprecedented mechanical strength are fabricated by complexation of polyacrylic acid(PAA),polyvinylpyrrolidone(PVPON),and carbonized polymer dots(CPDs)(denoted as PAA-PVPON-CPDs).The incorporation of 15 wt%CPDs generates PAA-PVPON-CPDs compositeswith a tensile strength of∼158 MPa and Young’s modulus of∼8.2GPa.Servingas nanofillers,theCPDs can establish strong interactions with polymers in PAA-PVPON composites.The CPDs and the in situ-formed PAAPVPON nanoparticles work in concert to significantly strengthen the PAA-PVPON-CPDs composites to an unprecedented strength.The PAA-PVPON-CPDs composites exhibit excellent impact resistance and damage tolerance because of the high mechanical strength of the composites and the energy dissipation mechanism of the CPDs and PAA-PVPON nanoparticles.Moreover,the fractured PAA-PVPON-CPDs composites can be healed to restore their original mechanical strength.
基金funded in part by the National Natural Science Foundation (No.30670199,30870180 and 30770185)the Zhejiang Scientific and Technological Program (No.2008C12081)+1 种基金the Hangzhou Scientific and Technological Program (No.20080432T06)Qianjiang Scholar Program
文摘Dendrobium plants are used commonly as tonic herbs and health food in many Asian countries, especially in China. Here we report the genetic map construction of two Dendrobium species with a double pseudo-testcross strategy using random amplified polymorphic DNA (RAPD) and sequence-related amplified polymorphism (SRAP) markers. A F1 mapping population of 90 individuals was developed from a cross between D. officinale and D. hercoglossum. A total of 307 markers, including 209 RAPD and 98 SRAP, were identified and used for genetic linkage group (LG) analysis. The D. officinale linkage map consisted of 11 major linkage groups and 3 doublets, which covered 629.4 cM by a total of 62 markers with an average locus distance of 11.2 cM between two adjacent markers. The D. hercoglos- sum linkage map contained 112 markers mapped on 15 major and 4 minor linkage groups, spanning a total length of 1,304.6 cM with an average distance of I 1.6 cM between two adjacent markers. The maps constructed in this study covered 92.7% and 82.7% of the D. hercoglossum and D. officinale genomes respectively, providing an important basis for the mapping of horticultural and medicinal traits and for the application of marker-assisted selection in Dendrobium breeding program.
基金financially supported by the National Natural Science Foundation of China(Nos.22077041 and 31770380)。
文摘Five novel heterodimers of cytochalasan and ergosterol,ergochaeglobosins A—E,were isolated from an endophytic fungus Chaetomium globosum P2-2-2.Ergochaeglobosin A(1) possesses an unprecedented 5/6/13/6/5/6/6/6 fused octacyclic ring system,and ergochaeglobosins B(2) and C(3) form a unique 5/6/13/6/6/6/6/5 fused octacyclic ring system,whereas ergochaeglobosins D(4) and F(5) are the first cytochalasan heterodimers formed via a N-1′/C-3′′single bond.Their structures with absolute configurations were established by extensive spectroscopic analyses,single-crystal X-ray diffraction,and ECD calculations.The plausible biogenetic pathway of 1—5 was postulated.Compound 1 exhibited inhibitory effects against ConA-induced T cells and LPS-induced B cells proliferation with IC50 values of 19.2 and 14.1μmol/L,respectively.Co-treatment of 3(20μmol/L)with TRAIL(150 ng/mL)could significantly decrease the cell viability of A549 by 24.9%comparing with monotherapy of 3(20μmol/L).
基金the National Natural Science Foundation of China(Nos.22105083 and 52173166)the Fundamental Research Funds for the Central Universities,JLU and JLUSTIRT(2017TD-06).
文摘Quasi-2D perovskites have been demonstrated to be competitive materials in the photodetection fields due to the enhanced moisture stability by large organic cations.However,as the increasing demands of modern technology,it is still challenging to combine the flexibility with the capability of weak light detection in a low-cost way.Here,amides,carboxylic acids,and anhydrides groups-rich carbonized polymer dots(CPDs)were employed to fll in the perovskite grain boundaries,which can passivate the point defects of perovskite by coordinating with the unbonded Pb atoms,and reduce the leakage current.Weak light detection capability was demonstrated by directly resolving light with an intensity of 10.1 pW cm^(-2).More importantly,the stretchable polymer chains on CPDs strongly interact with perovskite ions through multiple supramolecular interactions,and extend the stretchable properties to the perovskite/CPDs composites,which can maintain the integral structure stability during the deformation of perovskite crystals and restricted any crack by releasing the flm strain.Our fabricated devices show extraordinary flexible stability in the bending-dependent response tests.The viscoelasticity of CPDs improves the bending stability of the flexible quasi-2D perovskite photodetectors,and device performance shows no degradation after bending 10000 times,comparable or even outperforming the dominating flexible photodetectors.
基金GRF,Grant/Award Number:12200118National Natural Science Foundation of China,Grant/Award Number:91856127SKLP,Grant/Award Number:1920_P06。
文摘Sensitive differentiation of an enantiomer from its mirror image(ie,enantiodifferentiation),a perennial challenge for pharmaceutical production and disease diagnosis,is technically limited by the weak optical activity(OA)of enantiomers,mainly due to their dimensional mismatch with light wavelengths in the ultraviolet(UV)-visible region.Here we use silver chiral nanoparticles(Ag CNPs)with nominally sub-5 nm helical pitch(P)to amplify the OA of(20R,30R,40S)-riboflavin-50-phosphate sodium salts(RP),which have been found to indirectly affect metabolic processes,through the formation of an RP thin film(TF)covering a close-packed array of Ag CNPs.The OA of the RP in the deep-UV region can be amplified up to 80-fold,ascribed to the aggregation of RP in the TFs and the interactions between RP and the atomically chiral lattices at the CNPs'surfaces.The former contribution,not associated with the chiral Ag topographies,plays a dominant role by thickening the RP TFs,so that the observed amplification has no enantioselective dependence on the chirality of the Ag CNPs.This study extends progress in the sensitive detection of bio-enantiomers,which is highly desired for advanced bio-detection in disease diagnosis and production of single-enantiomer pharmaceuticals.
基金supported by the National Key R&D Program(No.2018YFD0200100)National Natural Science Foundation of China(Nos.21837001,21273089,22007035,U20A2038)+3 种基金the Open Project Fund of the Key Laboratory of the Pesticides and Chemical Biology of Central China Normal University(No.2018-A01)the Fundamental Research Funds for the South-Central University for Nationalities(No.CZW20020)the Fundamental Research Funds for the Central Universities(No.KJ02072020-0657)Hubei Province Natural Science Foundation(No.2020CFB487)。
文摘4-Hydroxyphenylpyruvate dioxygenase(HPPD)is an important target for both drug and pesticide discovery.As a typical Fe(II)-dependent dioxygenase,HPPD catalyzes the complicated transformation of 4-hydroxyphenylpyruvic acid(HPPA)to homogentisic acid(HGA).The binding mode of HPPA in the catalytic pocket of HPPD is a focus of research interests.Recently,we reported the crystal structure of Arabidopsis thaliana HPPD(At HPPD)complexed with HPPA and a cobalt ion,which was supposed to mimic the pre-reactive structure of At HPPD-HPPA-Fe(II).Unexpectedly,the present study shows that the restored At HPPD-HPPA-Fe(II)complex is still nonreactive toward the bound dioxygen.QM/MM and QM calculations reveal that the HPPA resists the electrophilic attacking of the bound dioxygen by the trim of its phenyl ring,and the residue Phe381 plays a key role in orienting the phenyl ring.Kinetic study on the F381 A mutant reveals that the HPPD-HPPA complex observed in the crystal structure should be an intermediate of the substrate transportation instead of the pre-reactive complex.More importantly,the binding mode of the HPPA in this complex is shared with several well-known HPPD inhibitors,suggesting that these inhibitors resist the association of dioxygen(and exert their inhibitory roles)in the same way as the HPPA.The present study provides insights into the inhibition mechanism of HPPD inhibitors.
基金supported by the National Natural Science Foundation of China(Nos.61074049,61273130)
文摘In this paper, we study stabilization for a Schoedinger equation, which is interconnected with a heat equation via boundary coupling. A direct boundary feedback control is adopted. By a detailed spectral analysis, it is found that there are two branches of eigenvalues: one is along the negative real axis, and the other is approaching to a vertical line, which is parallel to the imagine axis. Moreover, it is shown that there is a set of generalized eigenfunctions, which forms a Riesz basis for the energy state space. Finally, the spectrum-determined growth condition is held and the exponential stability of the system is then concluded.